During the last few decades, materials scientists have made notable advances in the development of ordered porous materials for catalysis, energy, separations, and biological applications. However, a key remaining challenge is the development of scalable techniques to manufacture self-standing hierarchically organized porous materials. State-of-the-art electrochemical devices (e.g. fuel cells, redox flow batteries, metal-air batteries) use porous materials with poorly defined three-dimensional microstructures, leading to limitations in performance. Novel applications require the development of materials with sophisticated control over the architecture at different length-scales. For example, selecting an adequate average pore size, porosity, and tortuosity would reduce pressure drop losses, improve mass transport and reaction distribution, decrease ohmic resistance, and maintain a low weight. We develop fabrication techniques to prepare architected materials with various degrees of hierarchical organization.